發(fā)布時(shí)間：2018-05-04 05:09

  本文選題：金屬有機(jī)骨架材料 + Cu-MOF　； 參考：《大連大學(xué)》2017年碩士論文

【摘要】：金屬有機(jī)骨架材料(MOFs)是一種新型多孔材料,因其比表面積大等特點(diǎn)而被廣泛應(yīng)用于催化、氣體吸附與分離等多種領(lǐng)域。在金屬有機(jī)骨架材料的合成過(guò)程中均需通過(guò)活化處理去除其結(jié)構(gòu)內(nèi)的客體分子并得到活性位點(diǎn)�，F(xiàn)有研究中大多采用加熱處理或者溶劑交換與加熱處理相結(jié)合的活化方式,分別稱為熱活化法和溶劑交換法。其中關(guān)于熱活化法已有相關(guān)研究討論了不同活化溫度的影響,而對(duì)于其他因素如活化氣氛的影響等未見(jiàn)報(bào)道。溶劑交換法雖然可有效去除孔道內(nèi)的客體分子,但活化過(guò)程所需時(shí)間較長(zhǎng)且需借助有機(jī)溶劑,如氯仿、甲醇等,存在污染和有毒問(wèn)題。本論文首先合成了一種銅基金屬有機(jī)骨架材料(Cu-MOF),采用X射線衍射儀(XRD)、N2吸附脫附、熱重測(cè)試(TG)及掃描電子顯微鏡(SEM)等對(duì)其晶體結(jié)構(gòu)、孔結(jié)構(gòu)、熱穩(wěn)定性及表面形貌等進(jìn)行了表征。結(jié)果表明合成的Cu-MOF是一種比表面積為1102.9m2·g-1的多孔材料,具有正八面體構(gòu)型,晶粒大小約為10μm,熱穩(wěn)定溫度約為300oC。其次,以自制的Cu-MOF為研究對(duì)象考察了熱活化過(guò)程中活化氣氛和活化溫度對(duì)其結(jié)構(gòu)和性能的影響。結(jié)果表明:活化氣氛對(duì)Cu-MOF的結(jié)構(gòu)及CO催化轉(zhuǎn)化活性有重要影響。在本實(shí)驗(yàn)所考察的四種活化氣氛(Ar、O2、CO標(biāo)準(zhǔn)氣及H2)中,O2及CO標(biāo)準(zhǔn)氣(1%CO、20%O2及79%N2)均可有效提高Cu-MOF的CO催化轉(zhuǎn)化活性,Ar及H2的活化作用則較弱。另一方面,活化溫度較低或過(guò)高均不能有效提高Cu-MOF的CO催化轉(zhuǎn)化活性。本實(shí)驗(yàn)所得最佳活化氣氛為CO標(biāo)準(zhǔn)氣,最佳熱活化溫度為240oC。此外,本論文還進(jìn)行了大氣壓冷等離子體活化Cu-MOF的相關(guān)研究,并以商品化Cu-MOF為載體負(fù)載過(guò)渡金屬,通過(guò)大氣壓冷等離子體進(jìn)行活化處理,考察了過(guò)渡金屬類型及負(fù)載量對(duì)樣品結(jié)構(gòu)和性能的影響。研究表明:(1)冷等離子體可有效降低Cu-MOF的CO起始轉(zhuǎn)化溫度;(2)負(fù)載不同過(guò)渡金屬對(duì)Cu-MOF的CO催化轉(zhuǎn)化活性有較大差異,在Fe、Co、Ni、Cu和Zn這五種過(guò)渡金屬中,負(fù)載Fe時(shí)樣品的CO催化轉(zhuǎn)化活性最高,且最佳負(fù)載量為7%。
[Abstract]:Organometallic skeleton (MOF) is a new porous material, which is widely used in many fields such as catalysis, gas adsorption and separation because of its large specific surface area. In the process of synthesis of organometallic skeleton materials, the active sites are obtained by removing the guest molecules in the structure of organometallic skeleton materials through activation treatment. Most of the existing researches use heating treatment or the combination of solvent exchange and heating treatment, which are called thermal activation method and solvent exchange method respectively. The influence of different activation temperature on the thermal activation method has been discussed, but the influence of other factors, such as the activation atmosphere, has not been reported. Although the solvent exchange method can effectively remove the guest molecules in the channels, the activation process takes a long time and requires organic solvents, such as chloroform, methanol, etc., which have the problems of pollution and toxicity. In this paper, a copper-base metal-organic skeleton material, Cu-MOF, was synthesized. The crystal structure, pore structure, thermal stability and surface morphology were characterized by X-ray diffractometer (XRD), thermogravimetric measurement (TG) and scanning electron microscopy (SEM). The results show that the synthesized Cu-MOF is a porous material with a specific surface area of 1102.9m2 g-1, with a normal octahedron configuration, a grain size of about 10 渭 m and a thermal stability temperature of about 300oC. Secondly, the effects of activation atmosphere and activation temperature on the structure and properties of Cu-MOF were investigated. The results show that the activation atmosphere has an important effect on the structure of Cu-MOF and the catalytic activity of CO. In the four activated atmospheres investigated in this experiment, the activity of CO catalytic conversion activity, ar and H _ 2, can be improved effectively by O _ 2 and CO _ (1) and CO _ (20) O _ 2 and 79N _ 2) in the four kinds of activated atmospheres, and H _ 2). On the other hand, low or too high activation temperature can not effectively improve the CO catalytic conversion activity of Cu-MOF. The best activation atmosphere is CO standard gas and the optimum thermal activation temperature is 240 OC. In addition, the paper also studied the activation of Cu-MOF by atmospheric pressure cold plasma. The commercial Cu-MOF was used as carrier to support transition metal, and the activated metal was treated by atmospheric cold plasma. The effects of transition metal type and loading amount on the structure and properties of the samples were investigated. The results show that the cold plasma can effectively reduce the CO conversion temperature of Cu-MOF. The catalytic activity of different transition metals for CO conversion of Cu-MOF is quite different. The CO catalytic conversion activity of the sample is the highest when Fe is loaded, and the optimum loading amount is 7%.
【學(xué)位授予單位】：大連大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：TB383.4;O643.36

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